Accurately engineering the electronic configuration of electrocatalysts to enhance their electrocatalytic performance is of importance in water splitting applications.Herein,a dual electronic regulation concept throug...Accurately engineering the electronic configuration of electrocatalysts to enhance their electrocatalytic performance is of importance in water splitting applications.Herein,a dual electronic regulation concept through constructing Fe-incorporated CoSe_(2)and Fe-incorporated Co_(9)S_(8)heterostructure nanorod arrays directly grown on a carbon cloth substrate(abbreviated as Fe-(CoSe_(2)/Co_(9)S_(8))@CC hereafter)is demonstrated.展开更多
Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the...Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the active centers hinder the further development of these catalysts.We here report a gasifiable reductant strategy,of which a new Cu-based metal organic framework(MOF:termed NTU-83)nanosheet was co-pyrolyzed with melamine to produce the N-coordinated atomic Cu and multi-oxidated Cu_(2+1)O active centers on the carbon foam with ultrathin skeleton.The engineered electrons and configuration of the active centers boost the catalyst(Cu/NC-1000)to show superior ORR activity(E_(1/2)=0.85 V),excellent stability,and methanol resistance.Further modeling calculation and controlled experiments reveal that the Cu_(2+1)O species play a crucial role in kinetically accelerated adsorption and activation of O_(2),while the N_(4)coordinated atomic Cu facilitates fast reduction of OH*.Such characteristics endow the Zn-air battery that containing Cu/NC-1000 as air cathode to show a high peak power density(138 mW·cm^(−2)),a high specific capacity of 763 mAh·gZn^(−1),and outstanding long-term cycle stability.The plausible mechanism and excellent performance show that gasifiable reductant strategy opens up a new route for regulation of the electronic of active sites but also provides a candidate for the practical application in energy conversion/storage devices.展开更多
基金supported by the National Natural Science Foundation of China(22302096)the Natural Science Foundation of Jiangsu Higher Education Institutions of China(23KJD150004)the High-level Talents Project of Jinling Institute of Technology(jit-b-202164).
文摘Accurately engineering the electronic configuration of electrocatalysts to enhance their electrocatalytic performance is of importance in water splitting applications.Herein,a dual electronic regulation concept through constructing Fe-incorporated CoSe_(2)and Fe-incorporated Co_(9)S_(8)heterostructure nanorod arrays directly grown on a carbon cloth substrate(abbreviated as Fe-(CoSe_(2)/Co_(9)S_(8))@CC hereafter)is demonstrated.
基金support from the National Natural Science Foundation of China(No.22171135)the Young and Middle-aged Academic Leader of Jiangsu Provincial Blue Project,the State Key Laboratory of Materials-Oriented Chemical Engineering(No.ZK201803)the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP).
文摘Efforts in a large number of transition metal-carbon systems are devoted to the development of efficient catalysts for oxygen reduction reaction(ORR).However,unsatisfied O_(2)adsorption and slow reduction of OH*at the active centers hinder the further development of these catalysts.We here report a gasifiable reductant strategy,of which a new Cu-based metal organic framework(MOF:termed NTU-83)nanosheet was co-pyrolyzed with melamine to produce the N-coordinated atomic Cu and multi-oxidated Cu_(2+1)O active centers on the carbon foam with ultrathin skeleton.The engineered electrons and configuration of the active centers boost the catalyst(Cu/NC-1000)to show superior ORR activity(E_(1/2)=0.85 V),excellent stability,and methanol resistance.Further modeling calculation and controlled experiments reveal that the Cu_(2+1)O species play a crucial role in kinetically accelerated adsorption and activation of O_(2),while the N_(4)coordinated atomic Cu facilitates fast reduction of OH*.Such characteristics endow the Zn-air battery that containing Cu/NC-1000 as air cathode to show a high peak power density(138 mW·cm^(−2)),a high specific capacity of 763 mAh·gZn^(−1),and outstanding long-term cycle stability.The plausible mechanism and excellent performance show that gasifiable reductant strategy opens up a new route for regulation of the electronic of active sites but also provides a candidate for the practical application in energy conversion/storage devices.
